Eu3+ ions activated La2Ti2O7 (La2Ti2O7:xEu3+) phosphors have been successfully synthesized by a fractional precipitation method from commercially available La2O3, Eu2O3, HNO3, Ti(SO4)2·9H2O and NH3·H2O as the starting materials. Detailed characterizations of the synthetic products were obtained by fourier transform infrared spectroscopy (FT-IR), X-ray diffractometry (XRD), differential thermal analysis, thermogravimetry and derivative thermogravimetry (DTA-TG-DTG), transmission electron microscopy (TEM), and photoluminescence (PL) spectroscopy. The results show that the precursor is composed of amorphous particles with quasi-spherical in shape and about 50 nm in size. Moreover, the precursor could be converted into pure La2Ti2O7 phase by calcining at 1000 °C for 2 h in air. The as-synthesized La2Ti2O7 particles are approximate polyhedron in shape and about 100–200 nm in size. PL spectroscopy of La2Ti2O7:xEu3+ phosphors reveals that the strongest emission peak is located at 616 nm under 275 nm ultraviolet (UV) light excitation, which corresponds to the 5D0→7F2 transition of Eu3+ ions. The quenching concentration of Eu3+ ions is 10.0 mol%, and its corresponding fluorescence lifetime was 1.82 ms according to the linear fitting result. Decay study reveals that the 5D0→7F2 transition of Eu3+ ions has a single exponential decay behavior.